CN108602995A - 阻燃性聚烯烃系树脂组合物 - Google Patents
阻燃性聚烯烃系树脂组合物 Download PDFInfo
- Publication number
- CN108602995A CN108602995A CN201780010052.9A CN201780010052A CN108602995A CN 108602995 A CN108602995 A CN 108602995A CN 201780010052 A CN201780010052 A CN 201780010052A CN 108602995 A CN108602995 A CN 108602995A
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- Prior art keywords
- ingredient
- fire
- acid
- resin composition
- retardant polyolefin
- Prior art date
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- 239000003063 flame retardant Substances 0.000 title claims abstract description 70
- 229920005672 polyolefin resin Polymers 0.000 title claims abstract description 70
- 239000011342 resin composition Substances 0.000 title claims abstract description 45
- 239000004615 ingredient Substances 0.000 claims abstract description 70
- NBIIXXVUZAFLBC-UHFFFAOYSA-N Phosphoric acid Chemical compound OP(O)(O)=O NBIIXXVUZAFLBC-UHFFFAOYSA-N 0.000 claims abstract description 31
- GLUUGHFHXGJENI-UHFFFAOYSA-N Piperazine Chemical compound C1CNCCN1 GLUUGHFHXGJENI-UHFFFAOYSA-N 0.000 claims abstract description 29
- 150000001875 compounds Chemical class 0.000 claims abstract description 18
- 229920000877 Melamine resin Polymers 0.000 claims abstract description 17
- 235000011007 phosphoric acid Nutrition 0.000 claims abstract description 16
- JDSHMPZPIAZGSV-UHFFFAOYSA-N melamine Chemical compound NC1=NC(N)=NC(N)=N1 JDSHMPZPIAZGSV-UHFFFAOYSA-N 0.000 claims abstract description 14
- 229920000137 polyphosphoric acid Polymers 0.000 claims abstract description 11
- 150000007974 melamines Chemical class 0.000 claims abstract description 10
- XZTOTRSSGPPNTB-UHFFFAOYSA-N phosphono dihydrogen phosphate;1,3,5-triazine-2,4,6-triamine Chemical compound NC1=NC(N)=NC(N)=N1.OP(O)(=O)OP(O)(O)=O XZTOTRSSGPPNTB-UHFFFAOYSA-N 0.000 claims abstract description 10
- MWFNQNPDUTULBC-UHFFFAOYSA-N phosphono dihydrogen phosphate;piperazine Chemical compound C1CNCCN1.OP(O)(=O)OP(O)(O)=O MWFNQNPDUTULBC-UHFFFAOYSA-N 0.000 claims abstract description 10
- 150000004885 piperazines Chemical class 0.000 claims abstract description 7
- 229920005989 resin Polymers 0.000 claims description 44
- 239000011347 resin Substances 0.000 claims description 44
- XLOMVQKBTHCTTD-UHFFFAOYSA-N Zinc monoxide Chemical compound [Zn]=O XLOMVQKBTHCTTD-UHFFFAOYSA-N 0.000 claims description 19
- 125000000217 alkyl group Chemical group 0.000 claims description 19
- OKTJSMMVPCPJKN-UHFFFAOYSA-N Carbon Chemical compound [C] OKTJSMMVPCPJKN-UHFFFAOYSA-N 0.000 claims description 17
- 239000003963 antioxidant agent Substances 0.000 claims description 15
- 230000003078 antioxidant effect Effects 0.000 claims description 15
- 229910052799 carbon Inorganic materials 0.000 claims description 14
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- 229920000098 polyolefin Polymers 0.000 claims description 10
- 239000011787 zinc oxide Substances 0.000 claims description 9
- ISIJQEHRDSCQIU-UHFFFAOYSA-N tert-butyl 2,7-diazaspiro[4.5]decane-7-carboxylate Chemical compound C1N(C(=O)OC(C)(C)C)CCCC11CNCC1 ISIJQEHRDSCQIU-UHFFFAOYSA-N 0.000 claims description 6
- YZCKVEUIGOORGS-IGMARMGPSA-N Protium Chemical compound [1H] YZCKVEUIGOORGS-IGMARMGPSA-N 0.000 claims 1
- 125000004435 hydrogen atom Chemical group [H]* 0.000 claims 1
- 239000000805 composite resin Substances 0.000 abstract description 2
- -1 nitrogenous compound Chemical class 0.000 description 58
- 239000002585 base Substances 0.000 description 25
- MTHSVFCYNBDYFN-UHFFFAOYSA-N diethylene glycol Chemical compound OCCOCCO MTHSVFCYNBDYFN-UHFFFAOYSA-N 0.000 description 24
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- RNFJDJUURJAICM-UHFFFAOYSA-N 2,2,4,4,6,6-hexaphenoxy-1,3,5-triaza-2$l^{5},4$l^{5},6$l^{5}-triphosphacyclohexa-1,3,5-triene Chemical compound N=1P(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP(OC=2C=CC=CC=2)(OC=2C=CC=CC=2)=NP=1(OC=1C=CC=CC=1)OC1=CC=CC=C1 RNFJDJUURJAICM-UHFFFAOYSA-N 0.000 description 16
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- 230000000694 effects Effects 0.000 description 13
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- 239000003795 chemical substances by application Substances 0.000 description 9
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- KKEYFWRCBNTPAC-UHFFFAOYSA-N Terephthalic acid Chemical compound OC(=O)C1=CC=C(C(O)=O)C=C1 KKEYFWRCBNTPAC-UHFFFAOYSA-N 0.000 description 8
- 239000000194 fatty acid Substances 0.000 description 8
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- 229920002545 silicone oil Polymers 0.000 description 8
- 239000004593 Epoxy Substances 0.000 description 7
- DGAQECJNVWCQMB-PUAWFVPOSA-M Ilexoside XXIX Chemical compound C[C@@H]1CC[C@@]2(CC[C@@]3(C(=CC[C@H]4[C@]3(CC[C@@H]5[C@@]4(CC[C@@H](C5(C)C)OS(=O)(=O)[O-])C)C)[C@@H]2[C@]1(C)O)C)C(=O)O[C@H]6[C@@H]([C@H]([C@@H]([C@H](O6)CO)O)O)O.[Na+] DGAQECJNVWCQMB-PUAWFVPOSA-M 0.000 description 7
- CPLXHLVBOLITMK-UHFFFAOYSA-N Magnesium oxide Chemical compound [Mg]=O CPLXHLVBOLITMK-UHFFFAOYSA-N 0.000 description 7
- 229910019142 PO4 Inorganic materials 0.000 description 7
- 235000014113 dietary fatty acids Nutrition 0.000 description 7
- 229930195729 fatty acid Natural products 0.000 description 7
- 235000011187 glycerol Nutrition 0.000 description 7
- 239000001257 hydrogen Substances 0.000 description 7
- 229910052739 hydrogen Inorganic materials 0.000 description 7
- 239000002667 nucleating agent Substances 0.000 description 7
- 239000002530 phenolic antioxidant Substances 0.000 description 7
- 235000021317 phosphate Nutrition 0.000 description 7
- 229920000728 polyester Polymers 0.000 description 7
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- 229910052708 sodium Inorganic materials 0.000 description 7
- 229940083542 sodium Drugs 0.000 description 7
- GXURZKWLMYOCDX-UHFFFAOYSA-N 2,2-bis(hydroxymethyl)propane-1,3-diol;dihydroxyphosphanyl dihydrogen phosphite Chemical class OP(O)OP(O)O.OCC(CO)(CO)CO GXURZKWLMYOCDX-UHFFFAOYSA-N 0.000 description 6
- VYPSYNLAJGMNEJ-UHFFFAOYSA-N Silicium dioxide Chemical compound O=[Si]=O VYPSYNLAJGMNEJ-UHFFFAOYSA-N 0.000 description 6
- YSMRWXYRXBRSND-UHFFFAOYSA-N TOTP Chemical compound CC1=CC=CC=C1OP(=O)(OC=1C(=CC=CC=1)C)OC1=CC=CC=C1C YSMRWXYRXBRSND-UHFFFAOYSA-N 0.000 description 6
- GWEVSGVZZGPLCZ-UHFFFAOYSA-N Titan oxide Chemical compound O=[Ti]=O GWEVSGVZZGPLCZ-UHFFFAOYSA-N 0.000 description 6
- 125000001931 aliphatic group Chemical group 0.000 description 6
- 229910000147 aluminium phosphate Inorganic materials 0.000 description 6
- 239000012964 benzotriazole Substances 0.000 description 6
- 239000001273 butane Substances 0.000 description 6
- 238000002485 combustion reaction Methods 0.000 description 6
- 150000004665 fatty acids Chemical class 0.000 description 6
- 229910052751 metal Inorganic materials 0.000 description 6
- VLKZOEOYAKHREP-UHFFFAOYSA-N n-Hexane Chemical compound CCCCCC VLKZOEOYAKHREP-UHFFFAOYSA-N 0.000 description 6
- OFBQJSOFQDEBGM-UHFFFAOYSA-N n-pentane Natural products CCCCC OFBQJSOFQDEBGM-UHFFFAOYSA-N 0.000 description 6
- 230000000704 physical effect Effects 0.000 description 6
- 238000012545 processing Methods 0.000 description 6
- 239000012779 reinforcing material Substances 0.000 description 6
- VGGSQFUCUMXWEO-UHFFFAOYSA-N Ethene Chemical compound C=C VGGSQFUCUMXWEO-UHFFFAOYSA-N 0.000 description 5
- 239000005977 Ethylene Substances 0.000 description 5
- 239000006057 Non-nutritive feed additive Substances 0.000 description 5
- PPBRXRYQALVLMV-UHFFFAOYSA-N Styrene Chemical compound C=CC1=CC=CC=C1 PPBRXRYQALVLMV-UHFFFAOYSA-N 0.000 description 5
- WNLRTRBMVRJNCN-UHFFFAOYSA-N adipic acid Chemical compound OC(=O)CCCCC(O)=O WNLRTRBMVRJNCN-UHFFFAOYSA-N 0.000 description 5
- QRUDEWIWKLJBPS-UHFFFAOYSA-N benzotriazole Chemical compound C1=CC=C2N[N][N]C2=C1 QRUDEWIWKLJBPS-UHFFFAOYSA-N 0.000 description 5
- 235000010290 biphenyl Nutrition 0.000 description 5
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- ZUOUZKKEUPVFJK-UHFFFAOYSA-N phenylbenzene Natural products C1=CC=CC=C1C1=CC=CC=C1 ZUOUZKKEUPVFJK-UHFFFAOYSA-N 0.000 description 5
- 239000010452 phosphate Substances 0.000 description 5
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- OAICVXFJPJFONN-UHFFFAOYSA-N Phosphorus Chemical compound [P] OAICVXFJPJFONN-UHFFFAOYSA-N 0.000 description 4
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- IISBACLAFKSPIT-UHFFFAOYSA-N bisphenol A Chemical compound C=1C=C(O)C=CC=1C(C)(C)C1=CC=C(O)C=C1 IISBACLAFKSPIT-UHFFFAOYSA-N 0.000 description 4
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- DOIRQSBPFJWKBE-UHFFFAOYSA-N dibutyl phthalate Chemical compound CCCCOC(=O)C1=CC=CC=C1C(=O)OCCCC DOIRQSBPFJWKBE-UHFFFAOYSA-N 0.000 description 4
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- CXMXRPHRNRROMY-UHFFFAOYSA-N sebacic acid Chemical class OC(=O)CCCCCCCCC(O)=O CXMXRPHRNRROMY-UHFFFAOYSA-N 0.000 description 4
- 239000004575 stone Substances 0.000 description 4
- 125000002889 tridecyl group Chemical group [H]C([*])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])C([H])([H])[H] 0.000 description 4
- JYEUMXHLPRZUAT-UHFFFAOYSA-N 1,2,3-triazine Chemical group C1=CN=NN=C1 JYEUMXHLPRZUAT-UHFFFAOYSA-N 0.000 description 3
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- ANBFRLKBEIFNQU-UHFFFAOYSA-M potassium;octadecanoate Chemical compound [K+].CCCCCCCCCCCCCCCCCC([O-])=O ANBFRLKBEIFNQU-UHFFFAOYSA-M 0.000 description 1
- PYJBVGYZXWPIKK-UHFFFAOYSA-M potassium;tetradecanoate Chemical compound [K+].CCCCCCCCCCCCCC([O-])=O PYJBVGYZXWPIKK-UHFFFAOYSA-M 0.000 description 1
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- 238000007639 printing Methods 0.000 description 1
- 235000019260 propionic acid Nutrition 0.000 description 1
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- 125000001453 quaternary ammonium group Chemical group 0.000 description 1
- 150000003254 radicals Chemical class 0.000 description 1
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- GDESWOTWNNGOMW-UHFFFAOYSA-N resorcinol monobenzoate Chemical compound OC1=CC=CC(OC(=O)C=2C=CC=CC=2)=C1 GDESWOTWNNGOMW-UHFFFAOYSA-N 0.000 description 1
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- 125000000999 tert-butyl group Chemical group [H]C([H])([H])C(*)(C([H])([H])[H])C([H])([H])[H] 0.000 description 1
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- 150000003527 tetrahydropyrans Chemical group 0.000 description 1
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- KHPCPRHQVVSZAH-UHFFFAOYSA-N trans-cinnamyl beta-D-glucopyranoside Natural products OC1C(O)C(O)C(CO)OC1OCC=CC1=CC=CC=C1 KHPCPRHQVVSZAH-UHFFFAOYSA-N 0.000 description 1
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- 150000003918 triazines Chemical class 0.000 description 1
- RJIFVNWOLLIBJV-UHFFFAOYSA-N tributyl benzene-1,2,4-tricarboxylate Chemical compound CCCCOC(=O)C1=CC=C(C(=O)OCCCC)C(C(=O)OCCCC)=C1 RJIFVNWOLLIBJV-UHFFFAOYSA-N 0.000 description 1
- DQWPFSLDHJDLRL-UHFFFAOYSA-N triethyl phosphate Chemical compound CCOP(=O)(OCC)OCC DQWPFSLDHJDLRL-UHFFFAOYSA-N 0.000 description 1
- ZIBGPFATKBEMQZ-UHFFFAOYSA-N triethylene glycol Chemical compound OCCOCCOCCO ZIBGPFATKBEMQZ-UHFFFAOYSA-N 0.000 description 1
- 125000005591 trimellitate group Chemical group 0.000 description 1
- WVLBCYQITXONBZ-UHFFFAOYSA-N trimethyl phosphate Chemical compound COP(=O)(OC)OC WVLBCYQITXONBZ-UHFFFAOYSA-N 0.000 description 1
- FYGHSUNMUKGBRK-UHFFFAOYSA-N trimethylbenzene Natural products CC1=CC=CC(C)=C1C FYGHSUNMUKGBRK-UHFFFAOYSA-N 0.000 description 1
- XZZNDPSIHUTMOC-UHFFFAOYSA-N triphenyl phosphate Chemical compound C=1C=CC=CC=1OP(OC=1C=CC=CC=1)(=O)OC1=CC=CC=C1 XZZNDPSIHUTMOC-UHFFFAOYSA-N 0.000 description 1
- RYFMWSXOAZQYPI-UHFFFAOYSA-K trisodium phosphate Chemical compound [Na+].[Na+].[Na+].[O-]P([O-])([O-])=O RYFMWSXOAZQYPI-UHFFFAOYSA-K 0.000 description 1
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- 235000019354 vermiculite Nutrition 0.000 description 1
- 230000000007 visual effect Effects 0.000 description 1
- 238000005406 washing Methods 0.000 description 1
- 239000010456 wollastonite Substances 0.000 description 1
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- 125000005023 xylyl group Chemical group 0.000 description 1
- XSMMCTCMFDWXIX-UHFFFAOYSA-N zinc silicate Chemical compound [Zn+2].[O-][Si]([O-])=O XSMMCTCMFDWXIX-UHFFFAOYSA-N 0.000 description 1
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- 229910001928 zirconium oxide Inorganic materials 0.000 description 1
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Abstract
本发明提供具有优异的耐热性和优异的阻燃性的聚烯烃系树脂组合物,具体而言,提供一种阻燃性聚烯烃系树脂组合物,其是相对于聚烯烃系树脂含有(A)成分:选自正磷酸三聚氰胺、焦磷酸三聚氰胺及多聚磷酸三聚氰胺的组中的1种以上的三聚氰胺盐、(B)成分:选自正磷酸哌嗪、焦磷酸哌嗪及多聚磷酸哌嗪的组中的1种以上的哌嗪盐及(C)成分:通式〔1〕和/或通式〔2〕所表示的化合物而成的。关于通式〔1〕和/或通式〔2〕的具体内容,如本说明书中记载的那样。
Description
技术领域
本发明涉及树脂本来的物性没有受损、耐热性及阻燃性优异的阻燃性聚烯烃系树脂组合物。
背景技术
合成树脂在成型加工性、耐热性及力学特性等优异的基础上,具有低比重、轻重量这样的优点,被广泛用于膜、片材及结构部件等各种成型体。此外,进行了许多将合成树脂与其他聚合物共混而赋予耐冲击性或弹性等新的物性的尝试。
但是,以聚烯烃系树脂为代表的具有高可燃性的合成树脂由于在广泛的领域被经常使用,所以为了对这些树脂赋予阻燃性,阻燃剂的配合变得必要而不可或缺。作为这样的阻燃剂,已知以多磷酸或焦磷酸和含氮化合物的盐作为主要成分、且通过在燃烧时形成表面膨胀层(Intumescent)而抑制分解产物的扩散或传热并发挥阻燃性的膨胀系阻燃剂具有优异的阻燃性。
特别是在以家电或汽车的蓄电池周边等为代表的要求高耐热性及高阻燃性的用途中,要求特别高的性能。
一直以来,为了兼顾耐热性及阻燃性,提出了将膨胀系阻燃剂与抗氧化剂并用的技术(参照专利文献1、2及3),但根据并用的抗氧化剂的种类有时耐热性能不足、或者变得需要大量的添加。于是,要求在不添加大量的抗氧化剂的情况下耐热性及阻燃性优异的阻燃性聚烯烃系树脂组合物。
现有技术文献
专利文献
专利文献1:日本专利5503071号说明书
专利文献2:美国专利申请公开第2011/0092622号说明书
专利文献3:美国专利申请公开第2007/0176154号说明书
发明内容
发明所要解决的问题
因此,本发明的目的在于提供具有优异的耐热性和优异的阻燃性的聚烯烃系树脂组合物。
用于解决问题的手段
于是,本发明人们为了达成上述目的而进行了深入研究,结果完成了本发明。即,本发明提供一种阻燃性聚烯烃系树脂组合物,其是相对于聚烯烃系树脂含有下述(A)成分、(B)成分及(C)成分而成的。
(A)成分:选自正磷酸三聚氰胺、焦磷酸三聚氰胺及多聚磷酸三聚氰胺的组中的1种以上的三聚氰胺盐,
(B)成分:选自正磷酸哌嗪、焦磷酸哌嗪及多聚磷酸哌嗪的组中的1种以上的哌嗪盐,
(C)成分:下述通式〔1〕和/或下述通式〔2〕所表示的化合物,
[化学式1]
(R1、R2及R3分别独立地表示2价的碳数为1~3的烃基)
[化学式2]
(R4、R5及R6分别独立地表示2价的碳数为1~3的烃基,R7、R8及R9分别独立地表示氢原子或1价的碳数为1~4的烃基)
具体实施方式
以下,基于优选的实施方式对本发明的阻燃性聚烯烃系树脂组合物进行说明。本发明涉及一种阻燃性聚烯烃系树脂组合物。本发明中所谓阻燃性意味着下述的性质:物质不易着火,而且即使着火而持续燃烧,其速度也非常缓慢,或者其后会自己熄灭;优选意味着具有在按照实施例中记载的UL-94V标准的燃烧等级中至少V-2的等级,所谓阻燃性聚烯烃系树脂组合物意味着含有1种以上的阻燃剂成分和1种以上的聚烯烃系树脂的组合物。以下,对各成分依次进行说明。
首先,对本发明的阻燃性聚烯烃系树脂组合物中使用的聚烯烃系树脂进行说明。
作为本发明的阻燃性聚烯烃系树脂组合物中使用的聚烯烃系树脂,没有特别限制,例如可以列举出低密度聚乙烯、直链状低密度聚乙烯、高密度聚乙烯、等规聚丙烯、间规聚丙烯、半等规聚丙烯、聚丁烯、环烯烃聚合物、立构嵌段聚丙烯、聚-3-甲基-1-丁烯、聚-3-甲基-1-戊烯、聚-4-甲基-1-戊烯等α-烯烃聚合物、乙烯/丙烯嵌段或无规共聚物、乙烯-甲基丙烯酸甲酯共聚物、乙烯-醋酸乙烯酯共聚物等α-烯烃共聚物等。
本发明中,聚烯烃系树脂不论分子量、聚合度、密度、软化点、溶剂中的不溶成分的比例、立体规整性的程度、催化剂残渣的有无、作为原料的单体的种类或配合比率、聚合催化剂的种类(例如齐格勒催化剂、茂金属催化剂等)等如何均可以使用。
本发明中使用的聚烯烃系树脂的熔体流动指数(MFI)的值优选为3~60g/10min,更优选为5~40g/10min。若MFI的值低于3g/10min,则有时树脂加工变得困难,若超过60g/10min,则有时成型体的物性降低。
另外,本发明中的MFI的值依据ASTM D 1238、采用190℃、10kg的条件而测定。
本发明中,也可以使用聚烯烃系树脂与热塑性弹性体的聚烯烃聚合物合金。作为该聚合物合金中使用的热塑性弹性体,例如可以列举出苯乙烯系热塑性弹性体、聚烯烃系热塑性弹性体、聚氯乙烯系热塑性弹性体、聚氨酯系热塑性弹性体、聚酯系热塑性弹性体、聚酰胺系热塑性弹性体、反式聚异戊二烯系热塑性弹性体、氟橡胶系热塑性弹性体、氯化聚乙烯系热塑性弹性体等。
作为上述苯乙烯系热塑性弹性体,可以列举出苯乙烯和/或α-甲基苯乙烯与其他的单体(例如马来酸酐、苯基马来酰亚胺、甲基丙烯酸甲酯、丁二烯、丙烯腈等)的共聚物、例如丙烯腈-苯乙烯(AS)树脂、丙烯腈-丁二烯-苯乙烯(ABS)树脂、甲基丙烯酸甲酯-丁二烯-苯乙烯(MBS)树脂、耐热ABS树脂、苯乙烯-丁二烯-苯乙烯(SBS)树脂、丙烯腈-丙烯酸酯-苯乙烯(AAS)树脂、苯乙烯-马来酸酐(SMA)树脂、甲基丙烯酸酯-苯乙烯(MS)树脂、苯乙烯-异戊二烯-苯乙烯SIS)树脂、丙烯腈-乙丙橡胶-苯乙烯(AES)树脂、苯乙烯-丁二烯-丁烯-苯乙烯(SBBS)树脂、甲基丙烯酸甲酯-丙烯腈-丁二烯-苯乙烯(MABS)树脂等热塑性树脂、以及将这些丁二烯或异戊二烯的双键氢化而得到的苯乙烯-乙烯-丁烯-苯乙烯(SEBS)树脂、苯乙烯-乙烯-丙烯-苯乙烯(SEPS)树脂、苯乙烯-乙烯-丙烯(SEP)树脂、苯乙烯-乙烯-乙烯-丙烯-苯乙烯(SEEPS)树脂等氢化苯乙烯系弹性体树脂,它们可以单独使用,也可以以多种的混合物使用。
作为上述聚烯烃系热塑性弹性体,为碳数为2~20的α-烯烃聚合物或共聚物,具体而言可以列举出乙烯-丙烯树脂、乙烯-丁烯树脂、乙烯-己烯树脂、乙烯-甲基戊烯树脂、乙烯-辛烯树脂、丁烯树脂、丁烯-甲基戊烯树脂、甲基戊烯树脂、乙烯-醋酸乙烯酯树脂、乙烯-甲基丙烯酸树脂、乙烯-甲基丙烯酸甲酯树脂等,它们可以单独使用,也可以以多种的混合物使用。
作为上述聚烯烃系树脂,从树脂物性的方面出发,更优选为等规聚丙烯、间规聚丙烯、半等规聚丙烯、立构嵌段聚丙烯、乙烯/丙烯嵌段或无规共聚物等聚丙烯系树脂。
本发明中,聚烯烃系树脂的含量在本发明的阻燃性聚烯烃系树脂组合物中优选为35质量%到88质量%,更优选为40质量%到85质量%,进一步更优选为45质量%到80质量%。
另外,作为聚烯烃系树脂,在使用聚烯烃系树脂与热塑性弹性体的聚烯烃聚合物合金的情况下,上述的含量设定为聚烯烃聚合物合金的含量。
接着,对本发明的阻燃性聚烯烃系树脂组合物中使用的(A)成分的三聚氰胺盐进行说明。(A)成分的三聚氰胺盐作为阻燃剂成分被使用。(A)成分的三聚氰胺盐从正磷酸三聚氰胺、焦磷酸三聚氰胺及多聚磷酸三聚氰胺的组中选择,它们可以单独使用,也可以以混合物使用。它们中从阻燃性的方面出发,优选为焦磷酸三聚氰胺。在将它们以混合物使用的情况下,焦磷酸三聚氰胺的含有比例越高越优选。此外,焦磷酸三聚氰胺的焦磷酸与三聚氰胺的比以摩尔比计优选为1:1.5~1:2.5,进而最优选为1:2。
这些磷酸与三聚氰胺的盐也可以通过使分别对应的磷酸或磷酸盐与三聚氰胺反应而获得,本发明的(A)成分中使用的三聚氰胺盐优选为使正磷酸1三聚氰胺加热缩合而得到的焦磷酸三聚氰胺或多聚磷酸三聚氰胺,特别优选为焦磷酸三聚氰胺。
接着,对本发明的阻燃性聚烯烃系树脂组合物中使用的(B)成分的哌嗪盐进行说明。(B)成分的哌嗪盐作为阻燃剂成分被使用。(B)成分的哌嗪盐从正磷酸哌嗪、焦磷酸哌嗪及多聚磷酸哌嗪的组中选择,它们可以单独使用,也可以以混合物使用。它们中,从阻燃性的方面出发,优选为焦磷酸哌嗪,在以混合物使用的情况下,焦磷酸哌嗪的含有比例越高越优选。此外,焦磷酸哌嗪的焦磷酸与哌嗪的比以摩尔比计优选为1:0.5~1:1.5,进而最优选为1:1。
这些磷酸与哌嗪的盐可以通过使分别对应的磷酸或磷酸盐与哌嗪反应而获得,本发明的(B)成分中使用的哌嗪盐优选为使2正磷酸1哌嗪加热缩合而得到的焦磷酸哌嗪或多聚磷酸哌嗪,特别优选为焦磷酸哌嗪。
上述(A)成分的含量在本发明的阻燃性聚烯烃系树脂组合物中优选为3~29质量%,更优选为5~24质量%,进一步更优选为6~22质量%。另一方面,上述(B)成分的含量在本发明的阻燃性树脂组成中优选为9~46质量%,更优选为13~38质量%,进一步更优选为15~35质量%。
此外,关于上述(A)成分与上述(B)成分的合计含量,为了发挥优异的阻燃性,并且不损害树脂的物性,在本发明的阻燃性聚烯烃系树脂组合物中优选为15质量%~60质量%,更优选为20质量%~50质量%,进一步更优选为25质量%~45质量%。低于15质量%时,有时得不到充分的阻燃性,若超过60质量%,则有可能会损害树脂的物性。
此外,上述(A)成分与上述(B)成分的含有比率(质量基准)优选为(A)/(B)=20/80~50/50,进一步优选为(A)/(B)=30/70~50/50。
接着,对本发明的阻燃性聚烯烃系树脂组合物中使用的(C)成分进行说明。
本发明的阻燃性聚烯烃系树脂组合物中,作为(C)成分,可使用作为酚系抗氧化剂的下述通式〔1〕和/或下述通式〔2〕所表示的化合物。该化合物由于即使单独也具有充分的抗氧化能力,所以发挥作为一次抗氧化剂的作用。
[化学式3]
(R1、R2及R3分别独立地表示2价的碳数为1~3的烃基)
[化学式4]
(R4、R5及R6分别独立地表示2价的碳数为1~3的烃基,R7、R8及R9分别独立地表示氢原子或1价的碳数为1~4的烃基)
本发明中,作为酚系抗氧化剂,采用上述通式〔1〕及上述通式〔2〕所表示的化合物的理由如下所述。
酚系抗氧化剂在分子内具有酯键的情况下,由于在树脂的加工时一部分酯键断裂,变成低分子的物质挥发,所以不充分表现出抗氧化剂的效果。
酚系抗氧化剂中的低受阻或半受阻型的酚系抗氧化剂在树脂的加工时变化成醌结构后,容易引起偶联,无法表现出充分的抗氧化效果,而且产生树脂的着色。进而在受阻酚部位在1分子中为1个的情况下,由于不能充分发挥抗氧化剂的效果,所以需要多个该部位。
根据以上,作为酚系抗氧化剂,采用分子内不具有酯键的受阻型的酚系抗氧化剂、且受阻酚部位在1分子中为2个以上的上述通式〔1〕及上述通式〔2〕所表示的化合物。
在上述通式〔1〕中,作为R1、R2及R3所表示的2价的碳数为1~3的烃基,可以列举出直链或支链的亚烷基、直链或支链的亚链烯基、亚炔基。
作为直链的亚烷基,可以列举出-(CH2)n-(n为1~3的整数),作为支链的亚烷基,可以列举出-CH(CH3)-、-CH2(CH2CH3)-、-CH(CH3)CH2-、-CH2CH(CH3)-,作为直链的亚链烯基,可以列举出-CH=CH-、-CH=CH-CH2-、-CH2-CH=CH-,作为支链的亚链烯基,可以列举出-C(CH3)=CH-、-CH=C(CH3)-,作为亚炔基,可以列举出-C≡C-、-CH2-C≡C-、-C≡C-CH2-。
作为上述通式〔1〕所表示的化合物,可以列举出1,3,5-三(3,5-二叔丁基-4-羟基苄基)异氰脲酸酯、1,3,5-三(3,5-二叔丁基-4-羟基苯基乙基)异氰脲酸酯、1,3,5-三(3,5-二叔丁基-4-羟基苯基丙基)异氰脲酸酯等,它们可以单独使用,也可以将2种以上混合使用。它们中,优选包含1,3,5-三(3,5-二叔丁基-4-羟基苄基)异氰脲酸酯。
上述通式〔2〕中,作为R4、R5及R6所表示的2价的碳数为1~3的烃基,可以列举出与R1、R2及R3所表示的2价的碳数为1~3的烃基同样的基团。
作为R7、R8及R9所表示的1价的碳数为1~4的烃基,可以列举出直链或支链的烷基、直链或支链的链烯基、直链或支链的炔基。作为直链的烷基,可以列举出CH3-、CH3CH2-、CH3CH2CH2-、CH3CH2CH2CH2-,作为支链的烷基,可以列举出CH3(CH3)CH-、CH3(CH3)CH2CH2-、CH3CH2(CH3)CH-、(CH3)3C-,作为直链的链烯基,可以列举出CH2=CH-、CH2=CHCH2-、CH3CH=CH-、CH2=CHCH2CH2-、CH3CH=CHCH2-、CH3CH2CH=CH-,作为支链的链烯基,可以列举出CH(CH3)=CH-、CH2=C(CH3)-、CH2=C(CH3)CH2-、CH3C(CH3)=CH2-,作为炔基,可以列举出CH≡C-、CH≡CCH2-、CH3C≡C-、CH≡CCH2CH2-、CH2C≡CCH2-、CH2CH2C≡CH2-。
作为上述通式〔2〕所表示的化合物的例子,可以列举出1,3,5-三(3,5-二叔丁基-4-羟基苄基)-2,4,6-三甲基苯、1,3,5-三(3,5-二叔丁基-4-羟基苯基乙基)-2,4,6-三甲基苯、1,3,5-三(3,5-二叔丁基-4-羟基苯基丙基)-2,4,6-三甲基苯、1,3,5-三(3,5-二叔丁基-4-羟基苄基)-2,4,6-三乙基苯、1,3,5-三(3,5-二叔丁基-4-羟基苄基)-2,4,6-三丙基苯、1,3,5-三(3,5-二叔丁基-4-羟基苄基)-2,4,6-三丁基苯、1,3,5-三(3,5-二叔丁基-4-羟基苄基)苯等,它们可以单独使用,也可以将2种以上混合使用。它们中,优选包含1,3,5-三(3,5-二叔丁基-4-羟基苄基)-2,4,6-三甲基苯。
上述通式〔1〕所表示的化合物与上述通式〔2〕所表示的化合物可以单独使用,也可以以2种的组的混合使用,混合的情况下的比率可以是任意值。
本发明的阻燃性聚烯烃系树脂组合物中的(C)成分的含量优选为0.01~5质量%,更优选为0.05~3质量份,进一步更优选为0.07~1.5质量%。
在(C)成分的含量低于0.01质量%的情况下,耐热性不足,在含量超过5质量%时,无法得到含有5质量%时以上的耐热性,增量添加变得没有意义。
接着对本发明的阻燃性聚烯烃系树脂组合物中使用的(D)成分进行说明。
本发明的阻燃性聚烯烃系树脂组合物优选进一步包含亚磷酸系抗氧化剂作为(D)成分。(D)成分的亚磷酸系抗氧化剂通过与作为一次抗氧化剂的上述(C)成分并用,发挥表现出更高的耐热性能这样的作为二次抗氧化剂的作用。
作为本发明中使用的(D)成分的亚磷酸系抗氧化剂,没有特别限定,例如可以列举出亚磷酸三(壬基苯基)酯、三〔2-叔丁基-4-(3-叔丁基-4-羟基-5-甲基苯基硫基)-5-甲基苯基〕亚磷酸酯、亚磷酸十三烷基酯、辛基二苯基亚磷酸酯、二(癸基)单苯基亚磷酸酯、二(十三烷基)季戊四醇二亚磷酸酯、二(壬基苯基)季戊四醇二亚磷酸酯、双(2,4-二叔丁基苯基)季戊四醇二亚磷酸酯、双(2,6-二叔丁基-4-甲基苯基)季戊四醇二亚磷酸酯、双(2,4,6-三叔丁基苯基)季戊四醇二亚磷酸酯、双(2,4-二枯基苯基)季戊四醇二亚磷酸酯、四(十三烷基)异亚丙基二苯酚二亚磷酸酯、四(十三烷基)-4,4'-正亚丁基双(2-叔丁基-5-甲基苯酚)二亚磷酸酯、六(十三烷基)-1,1,3-三(2-甲基-4-羟基-5-叔丁基苯基)丁烷三亚磷酸酯、四(2,4-二叔丁基苯基)亚联苯基二亚膦酸酯、9,10-二氢-9-氧杂-10-磷杂菲-10-氧化物、2,2'-亚甲基双(4,6-叔丁基苯基)-2-乙基己基亚磷酸酯、2,2'-亚甲基双(4,6-叔丁基苯基)-十八烷基亚磷酸酯、2,2'-亚乙基双(4,6-二叔丁基苯基)氟代亚磷酸酯、三(2-〔(2,4,8,10-四叔丁基二苯并〔d,f〕〔1,3,2〕二噁磷环庚烷-6-基)氧〕乙基)胺、2-乙基-2-丁基丙二醇与2,4,6-三叔丁基苯酚的亚磷酸酯、三(2,4-二-叔丁基苯基)亚磷酸酯等。它们可以单独使用,也可以以2种以上的混合物使用。
它们中,优选为双(2,6-二叔丁基-4-甲基苯基)季戊四醇二亚磷酸酯、2,2’-亚甲基双(4,6-叔丁基苯基)-2-乙基己基亚磷酸酯、三(2,4-二叔丁基苯基)亚磷酸酯等。
本发明的阻燃性聚烯烃系树脂组合物中的(D)成分的含量在阻燃性聚烯烃系树脂组合物中优选为0.01~5质量%,更优选为0.05~3质量份,进一步更优选为0.07~1.5质量%。
接着对本发明的阻燃性聚烯烃系树脂组合物中使用的(E)成分进行说明。
本发明的阻燃性聚烯烃系树脂组合物优选进一步含有氧化锌(ZnO)作为(E)成分。该氧化锌作为阻燃剂成分被使用。该氧化锌也可以进行表面处理。氧化锌可以使用市售品,例如可以列举出氧化锌1种(三井金属矿业(株)制造)、部分被膜型氧化锌(三井金属矿业(株)制造)、Nanofine 50(平均粒径为0.02μm的超微粒氧化锌:堺化学工业(株)制造)、Nanofine K(平均粒径为0.02μm的硅酸锌被覆的超微粒氧化锌:堺化学工业(株)制造)等。它们可以单独使用,也可以将2种以上混合使用。
关于本发明的阻燃性聚烯烃系树脂组合物中的(E)成分的含量,从阻燃性的方面出发,相对于(A)成分与(B)成分的合计100质量份,优选为0.01~10质量份,更优选为0.5~10质量份,进一步更优选为1.0~7.5质量份。
进而,本发明的阻燃性聚烯烃系树脂组合物中,还优选根据需要配合润滑剂。作为这样的润滑剂,可以列举出液体石蜡、天然石蜡、微晶石蜡、合成石蜡、低分子量聚乙烯、聚乙烯蜡等纯烃系润滑剂;卤代烃系润滑剂;高级脂肪酸、羟基脂肪酸等脂肪酸系润滑剂;脂肪酸酰胺、双脂肪酸酰胺等脂肪酸酰胺系润滑剂;脂肪酸的低级醇酯、甘油酯等脂肪酸的多元醇酯、脂肪酸的聚乙二醇酯、脂肪酸的脂肪醇酯(酯蜡)等酯系润滑剂;金属皂、脂肪醇、多元醇、聚乙二醇、聚甘油、脂肪酸与多元醇的部分酯、脂肪酸与聚乙二醇、聚甘油的部分酯系的润滑剂、或硅油、矿物油等。
这些润滑剂的含量相对于聚烯烃系树脂100质量份优选为0.01~5质量份,更优选为0.05~3质量份。
本发明的阻燃性聚烯烃系树脂组合物中,为了提高加工性,还优选含有硅油作为加工助剂。作为硅油的例子,可以列举出聚硅氧烷的侧链、末端全部为甲基的二甲基硅油、聚硅氧烷的侧链的一部分为苯基的甲基苯基硅油、聚硅氧烷的侧链的一部分为氢的甲基氢硅油等、以及它们的共聚物,此外也可以使用在它们的侧链和/或末端的一部分中导入了有机基团而得到的、胺改性、环氧改性、脂环式环氧改性、羧基改性、甲醇改性、巯基改性、聚醚改性、长链烷基改性、氟烷基改性、高级脂肪酸酯改性、高级脂肪酸酰胺改性、硅烷醇改性、二醇改性、酚改性和/或芳烷基改性等的改性硅油。
若列举出上述硅油的具体例子,作为二甲基硅油,可以列举出KF-96(信越化学(株)制造)、KF-965(信越化学(株)制造)、KF-968(信越化学(株)制造)等,作为甲基氢硅油或具有甲基氢聚硅氧烷结构的硅油,可以列举出KF-99(信越化学(株)制造)、KF-9901(信越化学(株))、HMS-151(Gelest公司制造)、HMS-071(Gelest公司制造)、HMS-301(Gelest公司制造)、DMS-H21(Gelest公司制造)等,作为甲基苯基硅油的例子,可以列举出KF-50(信越化学(株)制造)、KF-53(信越化学(株)制造)、KF-54(信越化学(株)制造)、KF-56(信越化学(株)制造)等,作为环氧改性品,可以列举出例如X-22-343(信越化学(株)制造)、X-22-2000(信越化学(株)制造)、KF-101(信越化学(株)制造)、KF-102(信越化学(株)制造)、KF-1001(信越化学(株)制造)等,作为羧基改性品,可以列举出例如X-22-3701E(信越化学(株)制造),作为甲醇改性品,可以列举出例如X-22-4039(信越化学(株)制造)、X-22-4015(信越化学(株)制造)等,作为胺改性品,可以列举出例如KF-393(信越化学(株)制造)等。
此外,作为加工助剂的硅油的含量在本发明的阻燃性聚烯烃系树脂组合物中优选为0.01~10质量%,更优选为0.05~7质量%,进一步更优选为0.1~5质量%。
本发明的阻燃性聚烯烃系树脂组合物中,在不损害本发明的效果的范围内,根据需要可以进一步使用不含有卤素的有机或无机系的阻燃剂·阻燃助剂中的一种以上。作为这些阻燃剂·阻燃助剂,可以列举出含三嗪环的化合物、金属氢氧化物、磷酸酯系阻燃剂、缩合磷酸酯系阻燃剂、磷酸盐系阻燃剂、无机磷系阻燃剂、二烷基次膦酸盐、有机硅系阻燃剂、金属氧化物、硼酸化合物、膨胀性石墨、其他的无机系阻燃助剂、其他的有机系阻燃剂等。
作为上述含三嗪环的化合物,例如可以列举出三聚氰酸二酰胺、苯并胍胺、乙酰胍胺、邻苯二胍胺(phthalodiguanamine)、三聚氰胺氰脲酸酯、亚丁基二胍胺、降冰片烯二胍胺、亚甲基二胍胺、亚乙基双三聚氰胺、三亚甲基双三聚氰胺、四亚甲基双三聚氰胺、六亚甲基双三聚氰胺、1,3-亚己基双三聚氰胺等。
作为上述金属氢氧化物,可以列举出氢氧化镁、氢氧化铝、氢氧化钙、氢氧化钡、氢氧化锌、KISUMA 5A(协和化学工业(株)制氢氧化镁的商标)等。
作为上述磷酸酯系阻燃剂的例子,可以列举出例如磷酸三甲酯、磷酸三乙酯、磷酸三丁酯、磷酸三(丁氧基乙基)酯、磷酸三(氯乙基)酯、磷酸三(二氯丙基)酯、磷酸三苯酯、磷酸三甲苯酯、磷酸甲苯基二苯基酯、磷酸三(二甲苯基)酯、磷酸辛基二苯基酯、磷酸二甲苯基二苯基酯、磷酸三(异丙基苯基)酯、磷酸2-乙基己基二苯基酯、磷酸叔丁基苯基二苯基酯、双-(叔丁基苯基)苯基磷酸酯、三-(叔丁基苯基)磷酸酯、磷酸异丙基苯基二苯基酯、双-(异丙基苯基)二苯基磷酸酯、三-(异丙基苯基)磷酸酯等。
作为上述缩合磷酸酯系阻燃剂的例子,可以列举出1,3-亚苯基双(磷酸二苯酯)、1,3-亚苯基双(磷酸二(二甲苯基)酯)、双酚A双(磷酸二苯酯)等。
作为上述无机磷系阻燃剂,可以列举出红磷。
作为上述二烷基次膦酸盐,可以列举出二乙基次膦酸铝、二乙基次膦酸锌等。
作为上述其他的无机系阻燃助剂,可以列举出例如氧化钛、氧化铝、氧化镁、二氧化钛、水滑石等无机化合物及其表面处理品。作为其具体例子,可以使用例如TIPAQUE R-680(石原产业(株)制氧化钛的商标)、KYOWA MAG150(协和化学工业(株)制氧化镁的商标)、DHT-4A(水滑石:协和化学工业(株)制造)、ALCAMIZER 4(协和化学工业(株)制锌改性水滑石的商标)等各种市售品。
本发明的阻燃性聚烯烃系树脂组合物根据需要还可以配合硫醚系抗氧化剂、紫外线吸收剂、受阻胺系光稳定剂、抗老化剂等。
作为上述硫醚系抗氧化剂,可以列举出例如硫代二丙酸二月桂酯、硫代二丙酸二肉豆蔻酯、硫代二丙酸二硬脂酯等硫代二丙酸二烷基酯类、及季戊四醇四(β-烷基硫代丙酸酯)类。
这些硫醚系抗氧化剂的含量相对于聚烯烃系树脂100质量份优选为0.001~10质量份,更优选为0.05~5质量份。
作为上述紫外线吸收剂,可以列举出例如2,4-二羟基二苯甲酮、2-羟基-4-甲氧基二苯甲酮、2-羟基-4-辛氧基二苯甲酮、5,5’-亚甲基双(2-羟基-4-甲氧基二苯甲酮)等2-羟基二苯甲酮类;2-(2’-羟基-5’-甲基苯基)苯并三唑、2-(2’-羟基-3’,5’-二叔丁基苯基)-5-氯苯并三唑、2-(2’-羟基-3’-叔丁基-5’-甲基苯基)-5-氯苯并三唑、2-(2’-羟基-5’-叔辛基苯基)苯并三唑、2-(2’-羟基-3’,5’-二枯基苯基)苯并三唑、2,2’-亚甲基双(4-叔辛基-6-(苯并三唑基)苯酚)、2-(2’-羟基-3’-叔丁基-5’-羧基苯基)苯并三唑等2-(2’-羟基苯基)苯并三唑类;水杨酸苯基酯、间苯二酚单苯甲酸酯、2,4-二叔丁基苯基-3,5-二叔丁基-4-羟基苯甲酸酯、2,4-二叔戊基苯基-3,5-二叔丁基-4-羟基苯甲酸酯、十六烷基-3,5-二叔丁基-4-羟基苯甲酸酯等苯甲酸酯类;2-乙基-2’-乙氧基草酰苯胺、2-乙氧基-4’-十二烷基草酰苯胺等取代草酰苯胺类;乙基-α-氰基-β,β-二苯基丙烯酸酯、甲基-2-氰基-3-甲基-3-(对甲氧基苯基)丙烯酸酯等氰基丙烯酸酯类;2-(2-羟基-4-辛氧基苯基)-4,6-双(2,4-二叔丁基苯基)-均三嗪、2-(2-羟基-4-甲氧基苯基)-4,6-二苯基-均三嗪、2-(2-羟基-4-丙氧基-5-甲基苯基)-4,6-双(2,4-二叔丁基苯基)-均三嗪等三芳基三嗪类。
这些紫外线吸收剂的含量相对于聚烯烃系树脂100质量份优选为0.001~30质量份,更优选为0.05~10质量份。
作为上述受阻胺系光稳定剂,可以列举出例如2,2,6,6-四甲基-4-哌啶基硬脂酸酯、1,2,2,6,6-五甲基-4-哌啶基硬脂酸酯、2,2,6,6-四甲基-4-哌啶基苯甲酸酯、双(2,2,6,6-四甲基-4-哌啶基)癸二酸酯、双(1,2,2,6,6-四甲基-4-哌啶基)癸二酸酯、双(1-辛氧基-2,2,6,6-四甲基-4-哌啶基)癸二酸酯、四(2,2,6,6-四甲基-4-哌啶基)-1,2,3,4-丁烷四羧酸酯、四(1,2,2,6,6-五甲基-4-哌啶基)-1,2,3,4-丁烷四羧酸酯、双(2,2,6,6-四甲基-4-哌啶基)·二(十三烷基)-1,2,3,4-丁烷四羧酸酯、双(1,2,2,6,6-五甲基-4-哌啶基)·二(十三烷基)-1,2,3,4-丁烷四羧酸酯、双(1,2,2,4,4-五甲基-4-哌啶基)-2-丁基-2-(3,5-二叔丁基-4-羟基苄基)丙二酸酯、1-(2-羟基乙基)-2,2,6,6-四甲基-4-哌啶醇/琥珀酸二乙酯缩聚物、1,6-双(2,2,6,6-四甲基-4-哌啶基氨基)己烷/2,4-二氯-6-吗啉基-均三嗪缩聚物、1,6-双(2,2,6,6-四甲基-4-哌啶基氨基)己烷/2,4-二氯-6-叔辛基氨基-均三嗪缩聚物、1,5,8,12-四〔2,4-双(N-丁基-N-(2,2,6,6-四甲基-4-哌啶基)氨基)-均三嗪-6-基〕-1,5,8,12-四氮杂十二烷、1,5,8,12-四〔2,4-双(N-丁基-N-(1,2,2,6,6-五甲基-4-哌啶基)氨基)-均三嗪-6-基〕-1,5,8-12-四氮杂十二烷、1,6,11-三〔2,4-双(N-丁基-N-(2,2,6,6-四甲基-4-哌啶基)氨基)-均三嗪-6-基〕氨基十一烷、1,6,11-三〔2,4-双(N-丁基-N-(1,2,2,6,6-五甲基-4-哌啶基)氨基)-均三嗪-6-基〕氨基十一烷等受阻胺化合物。
这些受阻胺系光稳定剂的含量相对于聚烯烃系树脂100质量份优选为0.001~30质量份,更优选为0.05~10质量份。
作为上述抗老化剂,可以列举出萘胺系、二苯胺系、对苯二胺系、喹啉系、氢醌衍生物、单酚系、硫代双酚系、受阻酚系、亚磷酸酯系等抗老化剂。这些抗老化剂的含量相对于聚烯烃系树脂100质量份优选为0.001~10质量份,优选为0.05~5质量份。
本发明的阻燃性聚烯烃系树脂组合物中,在不损害本发明的效果的范围内,也可以配合增强材料作为任意成分。作为该增强材料,可以使用通常用于增强合成树脂的纤维状、板状、粒状、粉末状的材料。具体而言,可以列举出玻璃纤维、石棉纤维、碳纤维、石墨纤维、金属纤维、钛酸钾晶须、硼酸铝晶须、镁系晶须、硅系晶须、硅灰石、海泡石、石棉、矿渣纤维、硬硅钙石、硅磷灰石、石膏纤维、二氧化硅纤维、二氧化硅/氧化铝纤维、氧化锆纤维、氮化硼纤维、氮化硅纤维及硼纤维等无机纤维状增强材料、聚酯纤维、尼龙纤维、丙烯酸纤维、再生纤维素纤维、醋酸酯纤维、槿麻、苎麻、棉花、黄麻、麻、剑麻、亚麻、亚麻布、丝绸、马尼拉麻、甘蔗、木浆、纸屑、旧纸及羊毛等有机纤维状增强材料、玻璃薄片、非溶胀性云母、石墨、金属箔、陶瓷珠、粘土、云母、绢云母、沸石、膨润土、白云石、高岭土、微粉硅酸、长石粉、钛酸钾、火山灰中空球(shirasu balloon,也可以称为白砂泡球或白洲泡球)、碳酸钙、碳酸镁、硫酸钡、氧化钙、氧化铝、氧化钛、二氧化钛、硅酸铝、石膏、均密石英岩、片钠铝石及白土等板状或粒状的增强材料。这些增强材料可以用乙烯/醋酸乙烯酯共聚物等热塑性树脂、或环氧树脂等热固化性树脂进行了被覆或集束处理,也可以用氨基硅烷或环氧基硅烷等偶联剂等进行了处理。
本发明的阻燃性聚烯烃系树脂组合物中,在不损害本发明的效果的范围内,还可以配合层状硅酸盐作为任意成分。作为层状硅酸盐,可以列举出蒙脱石、皂石、锂蒙脱石、贝得石、硅镁石、绿脱石等蒙脱石系粘土矿物、蛭石、埃洛石、溶胀性云母、滑石等,其层间还可以插入有有机阳离子、季铵阳离子、鏻阳离子。
本发明的阻燃性聚烯烃系树脂组合物中,在不损害本发明的效果的范围内,还可以进一步配合成核剂作为任意成分。作为该成核剂,可以适当使用一般作为聚合物的成核剂使用的物质,本发明中,可以使用无机系成核剂及有机系成核剂中的任一者。
作为上述无机系成核剂的具体例子,可以列举出高岭石、合成云母、粘土、沸石、石墨、炭黑、氧化镁、氧化钛、硫化钙、氮化硼、碳酸钙、硫酸钡、氧化铝、氧化钕及苯基膦酸盐等金属盐。为了提高在组合物中的分散性,这些无机系成核剂也可以用有机物进行了改性。
作为上述有机系成核剂的具体例子,可以列举出苯甲酸钠、苯甲酸钾、苯甲酸锂、苯甲酸钙、苯甲酸镁、苯甲酸钡、对苯二甲酸锂、对苯二甲酸钠、对苯二甲酸钾、草酸钙、月桂酸钠、月桂酸钾、肉豆蔻酸钠、肉豆蔻酸钾、肉豆蔻酸钙、二十八烷酸钠、二十八烷酸钙、硬脂酸钠、硬脂酸钾、硬脂酸锂、硬脂酸钙、硬脂酸镁、硬脂酸钡、褐煤酸钠、褐煤酸钙、甲苯酸钠、水杨酸钠、水杨酸钾、水杨酸锌、二苯甲酸铝、二苯甲酸钾、二苯甲酸锂、β-萘二甲酸钠、环己烷甲酸钠等有机羧酸金属盐、对甲苯磺酸钠、磺基间苯二甲酸钠等有机磺酸盐、硬脂酰胺、亚乙基双月桂酰胺、棕榈酰胺、羟基硬脂酰胺、芥酸酰胺、均苯三酸三(叔丁基酰胺)等羧酰胺、亚苄基山梨糖醇及其衍生物、2,2'-亚甲基双(4,6-二-叔丁基苯基)磷酸钠等磷化合物金属盐及2,2-甲基双(4,6-二-叔丁基苯基)钠等。
在本发明的阻燃性聚烯烃系树脂组合物中,在不损害本发明的效果的范围内,还可以配合增塑剂作为任意成分。作为该增塑剂,可以适当使用一般作为聚合物的增塑剂使用的物质,可以列举出例如聚酯系增塑剂、甘油系增塑剂、多元羧酸酯系增塑剂、聚亚烷基二醇系增塑剂及环氧系增塑剂等。本发明中在使用这些增塑剂的情况下,可以仅使用1种,也可以将2种以上并用。
作为上述聚酯系增塑剂的具体例子,可以列举出由己二酸、癸二酸、对苯二甲酸、间苯二甲酸、萘二甲酸、联苯二甲酸、松香等酸成分与丙二醇、1,3-丁二醇、1,4-丁二醇、1,6-己二醇、乙二醇、二甘醇等二醇成分构成的聚酯;聚己内酯等由羟基羧酸构成的聚酯等。这些聚酯可用单官能羧酸或单官能醇将末端封端,另外可用环氧化合物等将末端封端。
作为上述甘油系增塑剂的具体例子,可以列举出甘油单乙酰单月桂酸酯、甘油二乙酰单月桂酸酯、甘油单乙酰单硬脂酸酯、甘油二乙酰单油酸酯及甘油单乙酰单褐煤酸酯等。
作为上述多元羧酸酯系增塑剂的具体例子,可以列举出邻苯二甲酸二甲酯、邻苯二甲酸二乙酯、邻苯二甲酸二丁酯、邻苯二甲酸二辛酯、邻苯二甲酸二庚酯、邻苯二甲酸二苄酯、邻苯二甲酸丁基苄基酯等邻苯二甲酸酯、偏苯三酸三丁酯、偏苯三酸三辛酯、偏苯三酸三己酯等偏苯三酸酯、己二酸二异癸酯、己二酸正辛基正癸基酯、己二酸甲基二甘醇丁基二甘醇酯、己二酸苄基甲基二甘醇酯、己二酸苄基丁基二甘醇酯等己二酸酯、乙酰柠檬酸三乙酯、乙酰柠檬酸三丁酯等柠檬酸酯、壬二酸二-2-乙基己酯等壬二酸酯、癸二酸二丁酯及癸二酸二-2-乙基己酯等癸二酸酯等。
作为上述聚亚烷基二醇系增塑剂的具体例子,可以列举出聚乙二醇、聚丙二醇、聚(环氧乙烷·环氧丙烷)嵌段和/或无规共聚物、聚四亚甲基二醇、双酚类的环氧乙烷加成聚合物、双酚类的环氧丙烷加成聚合物、双酚类的四氢呋喃加成聚合物等聚亚烷基二醇、或其末端环氧改性化合物、末端酯改性化合物、及末端醚改性化合物等、末端封端化合物等。
上述环氧系增塑剂一般是指由环氧硬脂酸烷基酯和大豆油形成的环氧三甘油酯等,此外还可以使用主要以双酚A和环氧氯丙烷为原料的所谓环氧树脂。
作为其他的增塑剂的具体例子,可以列举出新戊二醇二苯甲酸酯、二乙二醇二苯甲酸酯、三乙二醇二-2-乙基丁酸酯等脂肪族多元醇的苯甲酸酯、硬脂酰胺等脂肪酸酰胺、油酸丁酯等脂肪族羧酸酯、乙酰基蓖麻油酸甲酯、乙酰基蓖麻油酸丁酯等羟基酸酯、季戊四醇、各种山梨糖醇、聚丙烯酸酯及石蜡类等。
本发明的阻燃性聚烯烃系树脂组合物中,在不损害本发明的效果的范围内,还可以进一步配合丙烯酸系加工助剂作为任意成分。丙烯酸系加工助剂可以使用使(甲基)丙烯酸酯的1种聚合或使2种以上共聚而得到的物质。
此外,本发明的阻燃性聚烯烃系树脂组合物中,在不损害本发明的效果的范围内,还可以配合防滴落剂,从考虑了对环境的负荷的无卤素的观点出发,氟系防滴落剂的配合不优选,进而由于有可能降低无规共聚物聚丙烯所具有的物性,所以不优选。作为氟系防滴落剂的例子,可以列举出例如聚四氟乙烯、聚偏氟乙烯、聚六氟丙烯等氟系树脂或全氟甲磺酸钠盐、全氟正丁烷磺酸钾盐、全氟叔丁烷磺酸钾盐、全氟辛烷磺酸钠盐、全氟-2-乙基己烷磺酸钙盐等全氟链烷磺酸碱金属盐化合物或全氟链烷磺酸碱土类金属盐等。
此外,本发明的阻燃性聚烯烃系树脂组合物中,根据需要,在不损害本发明的效果的范围内可以配合通常在合成树脂中使用的添加剂、例如交联剂、抗静电剂、金属皂、填充剂、防雾剂、防结垢剂、表面处理剂、荧光剂、防霉剂、杀菌剂、发泡剂、金属钝化剂、脱模剂、颜料、加工助剂等。
本发明中在含有聚烯烃系树脂及(A)~(E)成分以外的任意成分的情况下,其含量只要是不损害本发明的效果的范围则没有特别限定,但相对于聚烯烃系树脂100质量份优选合计设定为40质量份以下,更优选设定为20重量份以下。
在制造本发明的阻燃性聚烯烃系树脂组合物时,使聚烯烃系树脂中含有上述(A)、(B)及(C)成分、根据需要进而含有上述(D)及(E)成分的时机没有特别限制。例如,可以预先将选自上述(A)~(E)成分中的2种以上复配化后配合到聚烯烃系树脂中,或者也可以相对于聚烯烃系树脂含有各个成分。
在复配化的情况下,可以将各成分预先分别粉碎后再混合,或者也可以预先将各成分混合后粉碎。配合聚烯烃系树脂以外的树脂或其他的任意成分的情况也同样。
本发明的成型体是将本发明的阻燃性聚烯烃系树脂组合物成型而得到的成型体。成型体的成型方法没有特别限定,可以列举出挤出加工、压延加工、注射成型、辊压成型、压缩成型、吹塑成型等,能够制造树脂板、片材、膜、异形品等各种形状的成型体。
本发明的阻燃性聚烯烃系树脂组合物及其成型体可以用于电气/电子/通信、农林水产、矿业、建设、食品、纤维、衣类、医疗、煤炭、石油、橡胶、皮革、汽车、精密设备、木材、建材、土木、家具、印刷、乐器等广泛的产业领域。更具体而言,可以用于打印机、电脑、文字处理机、键盘、PDA(小型信息终端机)、电话机、复印机、传真、ECR(电子式收银机)、计算器、电子笔记本、卡、架子、文具等办公用品、OA设备、洗衣机、冰箱、吸尘器、微波炉、照明器具、游戏机、电熨斗、被炉等家电设备、TV、VTR、摄像机、收录机、录音机、微型磁盘、CD播放器、扩音器、液晶显示器等AV设备、连接器、继电器、电容器、开关、印刷基板、线圈骨架、半导体密封材料、LED密封材料、电线、电缆、变压器、偏转轭、配电盘、钟表等电气/电子部件及通信设备、OA设备等的箱体(框架、框体、外壳、外包装)或部件、汽车内外装饰材料的用途。
进而,本发明的阻燃性聚烯烃系树脂组合物及其成型体可以用于座位(填充物、内饰件等)、带、顶篷、活顶车顶篷、扶手、车门内饰、后杂物箱、地毯、垫子、遮阳板、轮毂装饰罩、垫子罩、安全气囊、绝缘材料、吊环、吊环带、电线被覆材料、电绝缘材料、涂料、涂布材料、外部装潢材料、地板材料、角壁、地毯、壁纸、壁装饰材料、外装饰材料、内装饰材料、屋顶材料、甲板材料、壁材、柱材、铺板、围墙的材料、骨架及造型、窗户及门的型材、木瓦、板壁、阳台、露台、防音板、绝热板、窗户材料、汽车、混合动力车、电动车、车辆、船舶、航空器、建筑物、住宅及建筑用材料、或土木材料、衣料、窗帘、床单、胶合板、合成纤维板、绒毯、玄关垫、片材、桶、软管、容器、眼镜、包、盒子、护目镜、滑雪板、球拍、帐篷、乐器等生活用品、运动用品等各种用途。
实施例
以下通过实施例对本发明进行具体说明。但是,本发明不受以下的实施例的任何限制。另外,以下的实施例等中%只要没有特别记载则为质量基准。
〔实施例1~5及比较例1~5〕
按照下述表1记载的配方制备实施例及比较例的阻燃性烯烃系树脂组合物,用混合器搅拌30分钟后,在200~230℃下挤出而制造粒料,接着使用其在200~220℃下进行注射成型,得到60×30×2mm和127×12.7×1.6mm的2种试验片。使用这些试验片进行下述各种试验。将结果示于表1中。
<阻燃性UL-94V试验方法>
将127×12.7×1.6mm的试验片保持垂直,使下端接焰10秒钟燃烧器的火后,取走火焰,对试验片测定点着的火熄灭的时间。接着,在火熄灭的同时进行10秒钟第2次的接焰,与第1次同样地测定点着的火熄灭的时间。此外,对于试验片下方的棉花是否因落下的火种而着火也同时进行评价。
由第1次和第2次的燃烧时间、棉花着火的有无等,按照UL-94V标准确定燃烧等级。关于燃烧等级,V-0是最高的燃烧等级,随着成为V-1、V-2而阻燃性降低。但是,不符合V-0~V-2的等级中的任一者的情况设定为NR。本发明中V-2以下的试验片不耐受实际使用。
<色差(色调试验)>
将60×30×2mm的试验片放入150℃的烘箱中,每48小时依据JIS Z 8781进行测定,由其测定值算出色差ΔE*。试验片的颜色越恶化,ΔE*的值变得越大。本发明中,以ΔE*的值超过30时的时间实施评价。ΔE*的值超过30时的时间越长,耐着色性能越良好,ΔE*的值超过30时的时间越短,耐着色性能越不良。ΔE*的值超过30时的时间低于1100小时的试验片不耐受实际使用。
<光泽度测定>
将60×30×2mm的试验片放入150℃的烘箱中,每48小时依据JIS Z 8741进行测定。本发明中计测光泽度的值达到60%以下时的时间。光泽度的值降低的时间越长,耐热性越良好,光泽度的值降低的时间越短,耐热性越不良。光泽度的值降低的时间低于1000小时的试验片不耐受实际使用。
<裂纹>
将60×30×2mm的试验片放入150℃的烘箱中,每48小时通过目视确认裂纹的有无。计测至产生裂纹为止的时间。至产生裂纹为止的时间越长,耐热性越良好,至产生裂纹为止的时间越短,耐热性越不良。本发明中低于800小时的试验片不耐受实际使用。
表1
*1:嵌段聚丙烯树脂(MFI=30g/10min)
*2:焦磷酸三聚氰胺:焦磷酸与三聚氰胺的比以摩尔比计为1∶2
*3:焦磷酸哌嗪:焦磷酸与哌嗪的比以摩尔比计为1∶1
*4:A0-20(株式会社艾迪科制):1.3.5-三(3.5-二叔丁基-4-羟基苄基)异氰脲酸酯
*5:A0-330(株式会社艾迪科制):1.3.5-三(3.5-二叔丁基-4-羟基苄基)-2.4.6-三甲基苯
*6:低受阻型:1.1.3-三(2-甲基-4-羟基-5-叔丁基苯基)丁烷
*7:酯型:四(3-(3.5-二叔丁基-4-羟基苯基)丙酸甲基)甲烷
*8:半受阻酯型:3.9-双(1.1-二甲基-2-{(3-叔丁基-4-羟基-5-甲基苯基)丙酰氧基}乙基)-2.4.8.10-四氧杂螺(5.5)十一烷
*9:双(2.6-二叔丁基-4-甲基苯基)季戊四醇二亚磷酸酯
*10:三(2.4-二叔丁基苯基)亚磷酸酯
*11:2.2.6.6-四甲基-4-哌啶基硬脂酸酯
*12:2-羟基-4-辛氧基二苯甲酮
产业上的可利用性
根据本发明,能够提供具有优异的耐热性和优异的阻燃性的聚烯烃系树脂组合物。
Claims (5)
1.一种阻燃性聚烯烃系树脂组合物,其是相对于聚烯烃系树脂含有下述(A)成分、(B)成分及(C)成分而成的,
(A)成分:选自正磷酸三聚氰胺、焦磷酸三聚氰胺及多聚磷酸三聚氰胺的组中的1种以上的三聚氰胺盐,
(B)成分:选自正磷酸哌嗪、焦磷酸哌嗪及多聚磷酸哌嗪的组中的1种以上的哌嗪盐,
(C)成分:下述通式〔1〕和/或下述通式〔2〕所表示的化合物,
R1、R2及R3分别独立地表示2价的碳数为1~3的烃基,
R4、R5及R6分别独立地表示2价的碳数为1~3的烃基,R7、R8及R9分别独立地表示氢原子或1价的碳数为1~4的烃基。
2.根据权利要求1所述的阻燃性聚烯烃系树脂组合物,其中,进一步含有作为(D)成分的亚磷酸系抗氧化剂或作为(E)成分的氧化锌中的任一者或两者。
3.根据权利要求1所述的阻燃性聚烯烃系树脂组合物,其中,所述阻燃性聚烯烃系树脂组合物中的所述(A)、(B)及(C)成分的含量如下述所示,
(A)成分:3~29质量%,
(B)成分:9~46质量%,
(C)成分:0.01~5质量%。
4.根据权利要求2或3所述的阻燃性聚烯烃系树脂组合物,其中,所述阻燃性聚烯烃系树脂组合物中的所述(D)及(E)成分的含量如下所示,
(D)成分:0.01~5质量%,
(E)成分:相对于所述(A)成分和(B)成分的合计100质量份为0.01~10质量份。
5.一种权利要求1~4中任一项所述的阻燃性聚烯烃系树脂组合物的成型体。
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WO2021002192A1 (ja) * | 2019-07-02 | 2021-01-07 | 株式会社Adeka | 耐熱安定助剤および耐熱安定剤組成物 |
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CN116323782A (zh) * | 2020-10-08 | 2023-06-23 | 株式会社艾迪科 | 聚烯烃系树脂组合物、使用其的成型品、及聚烯烃系树脂组合物的制造方法 |
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BR112018015727A2 (pt) | 2019-01-08 |
EP3444300B1 (en) | 2020-11-18 |
CN108602995B (zh) | 2021-06-22 |
KR20180135879A (ko) | 2018-12-21 |
BR112018015727B8 (pt) | 2022-08-16 |
JPWO2017179289A1 (ja) | 2019-02-21 |
WO2017179289A1 (ja) | 2017-10-19 |
BR112018015727B1 (pt) | 2022-07-05 |
EP3444300A4 (en) | 2019-11-13 |
JP6901467B2 (ja) | 2021-07-14 |
EP3444300A1 (en) | 2019-02-20 |
US20190040245A1 (en) | 2019-02-07 |
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